Classifications

• • C—CHEMISTRY; METALLURGY
  • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
  • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
  • C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
  • C04B28/02—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing hydraulic cements other than calcium sulfates
  • C04B28/04—Portland cements
• • C—CHEMISTRY; METALLURGY
  • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
  • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
  • C04B38/00—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof
  • C04B38/08—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof by adding porous substances
  • C04B38/085—Porous mortars, concrete, artificial stone or ceramic ware; Preparation thereof by adding porous substances of micro- or nanosize
• • C—CHEMISTRY; METALLURGY
  • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
  • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
  • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
  • C04B2111/00017—Aspects relating to the protection of the environment
• • C—CHEMISTRY; METALLURGY
  • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
  • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
  • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
  • C04B2111/10—Compositions or ingredients thereof characterised by the absence or the very low content of a specific material
• • C—CHEMISTRY; METALLURGY
  • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
  • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
  • C04B2201/00—Mortars, concrete or artificial stone characterised by specific physical values
  • C04B2201/50—Mortars, concrete or artificial stone characterised by specific physical values for the mechanical strength

Definitions

• Photocatalytic technology within concrete matrix is widely plebiscite to overcome urban NO x pollutants.
• such technologies rely on the functionalization of concrete with expensive, nonrenewable, nanosized photocatalytic oxides additives.
• pyrogenic carbonaceous material such as biochar offers not only equally effective but improved NO x mitigation performance at half the specific surface compared to activated carbon. Even more surprisingly it was found that when used at same addition rate biochar offers increased NO x absorption compared to activated carbon, even when used on concrete with higher porosity. In other words, the use of a pyrogenic carbonaceous material in a pervious concrete increases NO x absorption to a much higher extent than activated carbon.
• the invention thus relates to a pervious concrete based on:
• the invention further relates to a use of the pervious concrete of the invention for removing, at least in part, from the atmosphere gases and volatile compounds including nitrogen oxides, and preferably NO x , sulfur oxides, volatile organic compounds, ozone, carbon monoxide.
• the pervious concrete is then used as a construction material.
• the invention further relates to a method for preparing the pervious concrete of the invention, comprising mixing cement, pyrogenic carbonaceous material and aggregates with water and compacting the resulting composition.
• the water to cement ratio ranges from 0.25 to 0.50, preferably from 0.30 to 0.40.
• Biochar is obtained by the thermal decomposition of biomass at a temperature ranging from 350 to 1200°C, preferably from 350 to 800°C, more preferably from 400 to 750°C and even more preferably from 450°C to 700°C.
• the heat treatment is a pyrolysis carried out at a temperature of above 550°C, and advantageously below 750°C or 700°C.
• the pyrolysis is typically performed in an oxygen- reduced atmosphere.
• Oxygen-reduced atmosphere is understood as an atmosphere with oxygen content below 21%.
• pyrolysis is performed in an oxygen reduced atmosphere with less than 10% oxygen in the atmosphere.
• biomass feedstock is a non-woody biomass, including but not limited to agricultural residues including peat, a solid formed due to the accumulation of partially degraded biomass and contains highly varying fractions of ash-forming elements.
• NO x is shorthand for nitric oxide (NO) and nitrogen dioxide (NO 2 ), the nitrogen oxides that are most relevant for air pollution. These gases contribute to the formation of smog and acid rain, as well as affecting tropospheric ozone.
• concrete refers to a composition based on hydraulic binder, aggregates, water, and admixtures which sets and hardens by means of hydration reactions and processes and which, after hardening, retains its strength and stability even under water.
• concrete is as defined in the standard NF EN 206+A1:2016.
• a "pervious concrete” - also called “draining concrete” - is a concrete whose porosity, or volume of voids, is high enough and interconnected for water to flow through the void network.
• a pervious concrete generally has less fine aggregates and cement paste than conventional concrete.
• a pervious concrete element is generally prepared by mixing aggregates with a cement paste, filling a formwork or mold with the mixture and applying pressure to the upper surface of the concrete element to obtain a suitable filling of the formwork or mold as well as a flat top surface.
• the application of pressure to pervious concrete is generally referred to as concrete compaction and can be done manually or mechanically, for example by means of a shovel, roller, paver, etc.
• Pervious concretes are generally formulated so as to be only slightly compressible or even uncompressible, so as to preserve its high porosity even after compaction.
• Hydraulic Binder A hydraulic binder is a material which sets and hardens by hydration.
• Exemplary hydraulic binders are cements, or compositions comprising cement.
• the cement comprises Portland clinker and a source of calcium sulfate.
• the cement is preferably as defined in the standard NF-EN-197-1 of April 2012, or in the standard NF EN 197-5 published in May 2021.
• the cements defined in these standards are grouped in 6 different families: CEM I, CEM II, CEM III, CEM IV, CEM V and CEM VI.
• the cement can also be a CEM I, CEM II, CEM III, CEM IV, CEM V or a CEM VI to which mineral components are further added in a second preparation step.
• the cement may be any mineral binder that comprises Portland clinker optionally mixed with one or several mineral components as defined below.
• the cement may optionally further contain a calcium aluminate cement or a calcium sulfoaluminate cement, typically 10 wt.-% or less of a calcium aluminate cement or a calcium sulfoaluminate cement, if shorter setting times and higher early age strength development are for example required.
• a calcium aluminate cement or a calcium sulfoaluminate cement typically 10 wt.-% or less of a calcium aluminate cement or a calcium sulfoaluminate cement, if shorter setting times and higher early age strength development are for example required.
• Calcium sulphate used according to the present invention includes gypsum (calcium sulphate dihydrate, CaSO 4 .2H 2 O), hemi-hydrate (CaSO 4 .1/2H 2 O), anhydrite (anhydrous calcium sulphate, CaSOt) or a mixture thereof. Calcium sulphate produced as a by-product of certain industrial processes may also be used. Preferably, the calcium sulphate content ranges from 0% to 5% by weight of the cement.
• the mineral component may designate slag (for example, as defined in the European NF EN 197-1 Standard of April 2012, paragraph 5.2.2), pozzolanic materials (for example as defined in the European NF EN 197-1 Standard of April 2012, paragraph 5.2.3), fly ash (for example, as described in the European NF EN 197-1 Standard of April 2012, paragraph 5.2.4), calcined schists (for example, as described in the European NF EN 197-1 Standard of April 2012, paragraph 5.2.5), material containing calcium carbonate, for example limestone (for example, as defined in the European NF EN 197-1 Standard paragraph 5.2.6), limestone components (for example, as defined in the "Concrete” NF P 18-508 Standard), silica fume (for example, as defined in the European NF EN 197-1 Standard of April 2012, paragraph 5.2.7), siliceous components (for example, as defined in the "Concrete” NF P 18-509 Standard), metakaolin or mixtures thereof.
• the mineral component may also be ground construction demolition waste.
• siliceous components are ground glass, solid or hollow glass beads, glass granules, expanded glass powder.
• Admixture refers to a material other than water, aggregates, cement, mineral component and pyrogenic carbonaceous material, that is used as an ingredient of concrete composition to modify its freshly mixed, setting, or hardened properties, and that is added to the concrete composition before or during its mixing with water.
• admixture and “chemical admixture” will have the same meaning in the present disclosure.
• Superpasticizer As used herein, the term "superplasticizer” is to be understood as an admixture including both water reducing agents and superplasticizers as described in the book entitled “ Concrete Admixtures Handbook, Properties Science and Technology", V.S. Ramachandran, Noyes Publications, 1984 .
• a water reducing agent is defined as an admixture which typically reduces the amount of mixing water by 10 to 15% for a given workability.
• the water reducing agents include, for example lignosulfonates, hydroxycarboxylic acids, carbohydrates and other specialized organic compounds, e.g. glycerol, polyvinyl alcohol, sodium alumino-methyl-siliconate, sulfanilic acid and casein.
• Sodium polycarboxylates-polysulfonates and sodium polyacrylates may also be used.
• the derivatives of phosphonic acid may also be used.
• the required amount of super-plasticizer generally depends on the reactivity of the cement. The lower the reactivity, the smaller is the required amount of super-plasticizer. In order to reduce the total amount of alkaline salts, the super-plasticizer may be used as a calcium salt rather than as a sodium salt.
• Particle size distributions and particle sizes less than about 200 ⁇ m are measured using a Malvern MS2000 laser granulometer.
• Pyrogenic carbonaceous materials are known to have a reduced carbon footprint (CO 2 ) as compared with activated carbon, such as explained for instance in WO2023/227630 .
• the pyrogenic carbonaceous material is advantageously in the form of particles having a D 90 of 300 ⁇ m or less, advantageously a D 90 ranging from 5 to 200 ⁇ m, more advantageously from 5 to 150.
• the pyrogenic carbonaceous material is advantageously in the form of particles having a D 50 of 50 ⁇ m or less, advantageously a D 50 ranging from 2 to 25 ⁇ m.
• the pyrogenic carbonaceous material has preferably a specific surface area ranging from 300 to1000 m 2 /g, advantageously from 350 to 800 m 2 /g, preferably from 380 to 600 m 2 /g and even more preferably from 400 to 500 m 2 /g.
• the specific surface area is typically measured by the BET method.
• the pyrogenic carbonaceous material is preferably biochar.
• the pyrogenic carbonaceous material content in the pervious concrete ranges from 0.1 wt.-% to 5 wt.-%, preferably from 0.8 wt.-% to 3.0 wt.-%, preferably from 1.0 wt.-% to 2 wt.-%, relative to the total weight of the cement.
• the weight/weight ratio of pyrogenic carbonaceous material to cement preferably ranges from 0.1 to 5 %, more preferably from 0.8 to 2.0 %, even more preferably from 1.0 to 1.8%.
• the hydraulic binder comprises cement.
• the cement has the definition provided above.
• the cement as used in the invention may be any type of cement comprising Portland clinker.
• the cement used in the invention is selected from the cements readily available on the market.
• cement is selected from CEM I or CEM III, as defined in the standard EN197-1 of April 2012.
• the pervious concrete may also comprise an admixture, for example one of those described in the EN 934-2 standards as of September 2002, EN 934-3 standard as of November 2009 or EN 934-4 as of August 2009.
• Admixtures are in particular selected from plasticizer, superplasticizer, defoamers (see WO2012/001292 page 6 lines 13-23), anti-efflorescence agents (see WO2012/001292 page 6 lines 24 to page 7 line 4), viscosity modifying agents (see WO2012/001292 page 7 lines 5-14), activating agents, accelerators and/or retarders (see WO2012/001292 page 7 lines 15-21), and combinations thereof.
• the concrete comprises from 0.05% by weight to 2% by weight of admixtures selected from the group consisting of plasticizer, superplasticizer and mixtures thereof, relative to the total weight of cement.
• the admixture may be added to the cement, to the hydraulic binder, or to the water when preparing a concrete composition.
• the pervious concrete and hydraulic binder are essentially free of photocatalytic agents.
• photocatalytic agent is to be understood as any material suited to accelerate a chemical reaction under the action of light, for example, photocatalytic titanium dioxide.
• a material or composition is "essentially free of" a particular component when the component is present in a very low content, usually 5% by weight or less, compared to the total weight of the material, more especially below 1% by weight.
• a concrete is essentially free of photocatalytic agent when photocatalytic agent is typically present in the cement in an amount of less than 1 wt% or preferably 0.1 wt% of the total weight of cement. Even more preferably, no photocatalytic agent is present in the concrete.
• the diameter of the aggregates advantageously ranges from 2 mm to 14 mm, preferably from 2 mm or from 4 mm to 10 mm, more preferably from 2 mm or from 4 mm to 6 mm.
• their content is less than 10% by volume compared to the total volume of aggregates.
• the fresh composition for pervious concrete comprises, by kg per cubic meter:
• the water to cement ratio preferably ranges from 0.25 to 0.50, preferentially from 0.30 to 0.40.
• the porosity of the pervious concrete in the dried (hardened) state ranges from 10% to 50%, preferably from 15% to 40%, more preferably from 20% to 35%, expressed as a percentage with respect to the volume of the final hardened concrete.
• the compressive strength of the pervious concrete after 28 days ranges from 5 to 20 MPa.
• the invention relates to a method for preparing the pervious concrete of the invention, comprising mixing cement, pyrogenic carbonaceous material, admixtures, aggregates with water.
• the water to cement ratio ranges from 0.25 to 0.50, preferentially from 0.30 to 0.40.
• a premix composition for concrete is prepared during a first step wherein the cement, the pyrogenic carbonaceous, optionally chemical admixtures and aggregates are mixed.
• the concrete or mortar composition may be prepared in a subsequent step wherein water is added to the premix composition.
• the mixing is done using a conventional mixer at a concrete mixing plant or directly in a drum-truck mixer, for a mixing time usual in the field.
• the composition is placed, in particular poured into a mold or formwork, and compacted.
• the placing and compacting steps are advantageously carried out at least partly simultaneously.
• the concrete can be compacted using any type of tool, such as a screed or roller.
• the pervious concrete is then used as a construction material.
• Exemplary uses include but are not limited to the use as construction materials with limited load bearing capacity including building interior or exterior facades and elements, precast elements to be used as depolluting walls or pavement e.g. bicycle or pedestrian pavements.
• the invention also relates to a method for depolluting the atmosphere (at least in part), or for withdrawing NO x from the atmosphere (at least in part), comprising trapping, in particular absorbing, atmosphere gases and volatile compounds including nitrogen oxides, and preferably NO x , carbon monoxide, sulfur oxides, volatile organic compounds and ozone, more preferably NO x , even more preferably NO 2 , in a building or construction comprising the pervious concrete of the invention.
• the invention further relates to a method for depolluting the atmosphere (at least in part), or for withdrawing carbon monoxide and NO x from the atmosphere (at least in part) in a zone to be depolluted, comprising manufacturing a building or a construction located in the zone to be depolluted with the pervious concrete of the invention.
• the invention is also directed to the use of particulate pyrogenic carbonaceous material obtained from biomass pyrolysis, said pyrogenic carbonaceous material having a specific surface area ranging from 300 to1000 m 2 /g, as defined above, to withdraw gases and volatile compounds including nitrogen oxides, and preferably carbon monoxide, NO x , sulfur oxides, volatile organic compounds and ozone, more preferably NO x , even more preferably NO 2 , from the atmosphere, in a pervious concrete being based on:
• the particle size distribution is measured by laser particle size analysis, e.g. using a Malvern Mastersizer 3000 laser analyzer.
• Measurement is performed in ethanol.
• the light source is a red He-Ne laser (632 nm) and blue diode (466 nm).
• the optical model is the Mie model and the computing matrix of polydisperse type.
• the apparatus is calibrated before each work session using a standard sample (C10 silica, Sibelco) with known particle size curve. Measurement is carried out with the following parameters: pump rate 2300 rpm and stirrer speed of 800 rpm.
• the sample is positioned to obtain 10 to 20 % obscuration. Measurement is conducted after stabilization of obscuration. 80 % sonication is emitted for 1 minute to ensure de-agglomeration of the sample. After about 30 seconds (to evacuate any air bubbles) the sample is measured for 15 seconds (15000 images analysed). Without emptying the cell, the measurement is repeated at least twice to verify the stability of the result and evacuation of any bubbles.
• the particle size of sand is generally determined by screening.
• the BET Brunauer-Emmett-Teller surface area analysis is a physical measurement of specific surface area and porous network through gas adsorption analysis. An inert gas, nitrogen, is continuously flowed over the sample with increasing pressure. Specifically, the specific surface area of the various powders - in particular of the pyrogenic carbonaceous material, such as biochar - is measured as follows.
• a sample of powder (generally around 0.3 to 0.75 g) is used.
• a 9 cm 3 cell is used.
• the measuring assembly (cell+glass rod) is weighed. Then the sample is added into the cell.
• the assembly (cell+glass rod+sample) is weighed.
• the measuring cell is placed on a degassing unit, and the sample is degassed.
• the pressure to be reached is 25 to 30 mTorr. The duration to reach this pressure depends on the nature of the sample, the quantity of matter and the number of cells on the degassing unit.
• the degassing step makes it possible to remove any adsorption (H 2 O, CO, CO 2 , etc.) from the surface of the sample.
• the mass of the sample is obtained by subtracting the mass of the cell from the mass of the cell+degassed sample.
• the sample is then analyzed after placing it on the measurement unit.
• the analyzer is a 3 Flex, commercialized by the Micromeritics company.
• the measurement is based on the adsorption of nitrogen by the sample at a given temperature, in this case, the temperature of liquid nitrogen, that is -196° C.
• the apparatus measures the pressure of the reference cell in which the adsorbate is at its saturated vapour pressure and the pressure of the sample cell into which known volumes of adsorbate are injected.
• the resulting curve from these measurements is the adsorption isotherm.
• it is necessary to know the dead volume of the cell a measurement of this volume is therefore carried out with helium before the analysis.
• the mass of the sample calculated beforehand is entered as a parameter.
• the surface area is determined by the software by linear regression from the experimental curve.
• Mesopores are understood as pores having a diameter ranging from 2 to 50 nanometers. Micropores are understood as pores having a diameter of less than 2 nanometers.
• the volume of mesopores - V meso - as well as the volume of the micropores - V micro - is determined from the nitrogen adsorption/desorption isotherms using the BET method described above.
• the pore size distribution (PSD) is calculated from adsorption isotherms by using the KJS (Kruk-Jaroniec-Sayari) method.
• KJS Keruk-Jaroniec-Sayari
• the porosity measurement of concrete is carried out by using a cylindrical hardened concrete test specimen of 11 cm diameter and 22 cm height which is placed in a recipient of which the internal volume corresponded to the dimensions of the sample.
• the totality of the internal volume of the recipient is filled with water, the sample then being completely immersed in water.
• the porosity corresponds to the ratio between the volume of water added and the internal volume of the recipient.
• the porosity of a concrete is expressed by a percentage with respect to the volume of the final hardened concrete.
• the compressive strength is measured on a cylindrical sample having a diameter of 11 cm and a height of 22 cm according to the standard EN 12390-3: 2001 "Testing hardened concrete-Part 3: Compressive strength of test specimens ".
• NO x gas adsorption tests were performed using a fused quartz reactor (3.8dm3). The gas was injected into the reactor via 5 holes to homogenize the flow pattern.
• the NO/NO2 concentration inlet (respectively 768 ⁇ g/m3 NO and 478 ⁇ g/m3 NO 2 ) and oulet streams were controlled with an automatic NO x gas analyser (AC32M from Environêt SA, France).
• the mixed two gases were injected via a nitrogen carrier, with controlled relative humidity (45%).
• C 0 and C sample are the simultaneous concentrations of the pollutant, at the outlet of the bypass and of the reactor containing the solid sample, respectively.
• Samples were exposed in the chamber over a period of 24 hours.
• the size of the samples is 15cm*15cm*5cm with only the top surface exposed to the pollutants stream (all other surfaces are blocked with sealer).
• the performance can also be expressed as a percentage by summing/integrating the instantaneous mitigation value over twenty four hours.
• Examples are based on pervious concrete, where coarse aggregates occupy most of the pervious concrete volume.
• Limestone gravels in the range size of 2-6 mm or 4-6 mm were used as coarse aggregates.
• the mass ratio of coarse aggregate to the binder was fixed at 5:1.
• the water to cement ratio was 0.35.
• the activated carbons are prepared from peat and steam activated (SA2, Norit) or from lignite heat activated in a rotary earth furnace (HOK Mahleptiert, HOK ® Activated Lignite).
• the biochars are sourced from Valbois and Novocarbo (FC1C, FB1C, FO1B). Valbois biochar was received with 0-5mm size cuts range and was grinded to ⁇ 100 ⁇ m.
• the activated carbons A1 and A2, as well as biochars B1-B4 have been chemically characterized.
• Table 6 summarizes chemistry percentages of carbon (C), hydrogen (H), oxygen (O), nitrogen (N).
• Table 4 Chemical composition. Contents are expressed in % w/w. Bulk density is measured according to standard EN 1097-6 : 2014. Label Product ref.
• Dry materials aggregates, cement, biochar/activated carbon addition and powder admixture
• a Rayneri mixer bowl Dry materials (aggregates, cement, biochar/activated carbon addition and powder admixture) are weighted and introduced all together into a Rayneri mixer bowl.
• Blending is started when the water is introduced into the bowl for two minutes and thirty seconds at low speed (v1).
• the pervious concretes samples are compacted to obtain the targeted volume porosity.
• Pervious concretes were prepared following using the compositions depicted in Tables 5 and 6. The final porosity of the pervious concretes obtained is also indicated in these tables.
• Example 1 presents the results for absorption efficacy when used in concrete with a porosity of 22%
• example 2 investigates the absorption efficacy in concrete with a porosity of 32-35%.
• Example 1 Comparison of Norit SA2 and Biochars FC1C (Novocarbo) & Valbois (Bordet) at 22% of porosity with CEM III cement
• Figure 1 compares the NO 2 mitigation capacity for the samples from concrete samples of series 1.
• NO 2 mitigation performances are described below in table 7.
• the value of 0 in Specific Surface Area for reference example MD0-22% is arbitrary.
• Example 2 NO 2 mitigation performance: Comparison of a family of Novocarbo biochars and lignite originated activated carbon (HOK) at 32%-35% of porosity with CEM I cement.
• HOK activated carbon
• the pervious concretes MD0-32%, MDA2-32%, MDB1-32%, MDB2-32% and MDB3-32% were prepared targeting a 32-35% volume macro-porosity.
• Figure 2 compares the NO 2 mitigation capacity for the samples from concrete samples of series 2.
• NO 2 mitigation performances are described below in table 8.
• the value of 0 in Specific Surface Area for reference example MD0-22% is arbitrary.
• MDA2-32%, MDB1-32%, MDB2-32% and MDB3-32% samples are systematically more efficient than reference example MDO-32% (upper curve with black round hollow markers).

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• 2024
  • 2024-03-26 EP EP24305456.6A patent/EP4624441A1/fr active Pending
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  • 2025-03-25 WO PCT/EP2025/058188 patent/WO2025202234A1/fr active Pending

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